The fixation of atmospheric N to NH is an essential process for sustaining life. One grand challenge is to develop efficient catalysts to photofix N under ambient conditions. Herein we report an all-inorganic catalyst, Au nanocrystals anchored on ultrathin TiO nanosheets with oxygen vacancies. It can accomplish photodriven N fixation in the "working-in-tandem" pathway at room temperature and atmospheric pressure. The oxygen vacancies on the TiO nanosheets chemisorb and activate N molecules, which are subsequently reduced to NH by hot electrons generated from plasmon excitation of the Au nanocrystals. The apparent quantum efficiency of 0.82% at 550 nm for the conversion of incident photons to NH is higher than those reported so far. Optimizing the absorption across the overall visible range with the mixture of Au nanospheres and nanorods further enhances the N photofixation rate by 66.2% in comparison with Au nanospheres used alone. This work offers a new approach for the rational design of efficient catalysts toward sustainable N fixation through a less energy-demanding photochemical process compared to the industrial Haber-Bosch process.
Gold nanorods (NRs), pseudo-one-dimensional rod-shaped nanoparticles (NPs), have become one of the burgeoning materials in the recent years due to their anisotropic shape and adjustable plasmonic properties. With the continuous improvement in synthetic methods, a variety of materials have been attached around Au NRs to achieve unexpected or improved plasmonic properties and explore state-of-the-art technologies. In this review, we comprehensively summarize the latest progress on Au NRs, the most versatile anisotropic plasmonic NPs. We present a representative overview of the advances in the synthetic strategies and outline an extensive catalogue of Au-NR-based heterostructures with tailored architectures and special functionalities. The bottom-up assembly of Au NRs into preprogrammed metastructures is then discussed, as well as the design principles. We also provide a systematic elucidation of the different plasmonic properties associated with the Au-NR-based structures, followed by a discussion of the promising applications of Au NRs in various fields. We finally discuss the future research directions and challenges of Au NRs.
The magnetic plasmons of three-dimensional nanostructures have unique optical responses and special significance for optical nanoresonators and nanoantennas. In this study, we have successfully synthesized colloidal Au and AuAg nanocups with a well-controlled asymmetric geometry, tunable opening sizes, and normalized depths (h/ b, where h is depth and b is the height of the templating PbS nanooctahedrons), variable magnetic plasmon resonance, and largely enhanced second-harmonic generation (SHG). The most-efficient SHG of the bare Au nanocups is experimentally observed when the normalized depth h/b is adjusted to ∼0.78−0.79. We find that the average magnetic field enhancement is maximized at h/b = ∼0.65 and reveal that the maximal SHG can be attributed to the joint action of the optimized magnetic plasmon resonance and the "lightning-rod effect" of the Au nanocups. Furthermore, we demonstrate for the first time that the AuAg heteronanocups prepared by overgrowth of Ag on the Au nanocups can synergize the magnetic and electric plasmon resonances for nonlinear enhancement. By the tailoring of the dual resonances at the fundamental excitation and second-harmonic wavelengths, the far-field SHG intensity of the AuAg nanocups is enhanced 21.8fold compared to that of the bare Au nanocups. These findings provide a strategy for the design of nonlinear optical nanoantennas based on magnetic plasmon resonances and can lead to diverse applications ranging from nanophotonics to biological spectroscopy.
For the first time, the plasmonic gold bipyramids (Au BPs) are introduced to the PbS colloidal quantum dot (CQD) solar cells for improved infrared light harvesting. The localized surface plasmon resonance peaks of Au BPs matches perfectly with the absorption peaks of conventional PbS CQDs. Owing to the geometrical novelty of Au BPs, they exhibit significantly stronger far‐field scattering effect and near‐field enhancement than conventional plasmonic Au nanospheres (NSs). Consequently, device open‐circuit voltage (Voc) and short‐circuit current (Jsc) are simultaneously enhanced, while plasmonic photovoltaic devices based on Au NSs only achieve improved Jsc. The different effects and working mechanisms of these two Au nanoparticles are systematically investigated. Moreover, to realize effective broadband light harvesting, Au BPs and Au NSs are used together to simultaneously enhance the device optical and electrical properties. As a result, a significantly increased power conversion efficiency (PCE) of 9.58% is obtained compared to the PCE of 8.09% for the control devices due to the synergistic effect of the two plasmonic Au nanoparticles. Thus, this work reveals the intriguing plasmonic effect of Au BPs in CQD solar cells and may provide insight into the future plasmonic enhancement for solution‐processed new‐generation solar cells.
Ultrathin gold, palladium and platinum nanoframes are synthesized for monitoring reactions. Each nanoframe contains a gold nanobipyramid at its center.
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